ISSN 0040-5795, Theoretical Foundations of Chemical Engineering, 2008, Vol. 42, No. 3, pp. 257263. Pleiades Publishing, Ltd.

., 2008. Original Russian Text D.S. Aribike, O.A. Olafadehan, 2008, published in Teoreticheskie Osnovy Khimicheskoi Tekhnologii, 2008, Vol. 42, No. 3, pp. 269275.

Modeling of Fixed Bed Adsorption of Phenols on Granular Activated Carbon*

D. S. Aribike and O. A. Olafadehan
Department of Chemical Engineering, University of Lagos, Lagos, Nigeria e-mail: olafadehan@yahoo.com AbstractMathematical modeling of liquid phase adsorption of phenols in xed beds of granular activated carbon was investigated. The model considered the effects of axial diffusion in the uid, the external lm and internal diffusional mass transfer resistances of the particles, and the nonlinear adsorption isotherm of Freundlich. It was shown that the analysis of a complex multicomponent adsorption system could be simplied by converting it into a pseudo single-component adsorption system. This was achieved by lumping the concentrations of the components together as one single parameter, chemical oxygen demand. The resulting model equations were solved using the orthogonal collocation method and third-order semi-implicit RungeKutta method combined with a step-size adjustment strategy. Excellent agreement between simulated results and pilot plant data was obtained. Also, the breakthrough proles revealed the formation of a primary monomolecular layer on the adsorbent surface. DOI: 10.1134/S0040579508030056
*

INTRODUCTION

Fierce competition among process industries and the strong need to protect available markets posed serious challenges to chemical engineers. Fortunately, engineers have an ever-growing range of tools to meet the challenges. Modeling is one of such tools and the advent of fast computers has made its application in process engineering very interesting and rewarding. Secondly, the use of models makes the running of costly and time-consuming experiments unnecessary. Thus, modeling saves costs and compensates for time and effort used in developing and simulating models. For instance, mathematical models can be developed and simulated to predict breakthrough curves of adsorption systems, which are widely employed in riding industrial wastewater of organic pollutants. Fixed bed adsorption is widely used for purifying liquid mixtures, especially industrial waste efuents. In a little over two decades, granular activated carbon (GAC) was extensively used for waste and water treatment. This stirred up considerable interest in the study of multicomponent adsorption [19]. Thomas and Lombardi [10] investigated the binary adsorption of a benzenetoluene mixture in a xed bed of activated carbon, using simple semiempirical models applicable to constant pattern behavior. Cooney and Strusi [11] obtained an analytical solution for the concentration proles of two solutes with constant behavior. Their solution is applicable only to systems satisfying Glueckaufs pseudobinary isotherms. Gariepy and
*

Zwiebel [12] studied binary adsorption in xed beds, but their model neglected intraparticle diffusional resistance. Mathematical models resulting from adsorption systems may be solved using the orthogonal collocation method. The orthogonal collocation technique developed over two decades ago [13, 14] is particularly useful for solving boundary value problems and requires less computing time compared to standard nite difference methods. The method has been widely applied to the simulation of adsorption systems [1520]. The present work focuses on the development of a generalized mathematical model for the prediction of lumped concentration of phenolic compounds removed from industrial wastewater in a xed bed of activated carbon adsorbent. The multicomponent adsorption system will be rationalized into a pseudo mono-component system by lumping together the concentrations of the organic compounds. The model accounts for intraparticle and interphase mass transport as well as nonlinear adsorption. MATHEMATICAL MODEL The model describes the adsorption of many solutes from a owing liquid stream onto a xed bed of GAC particles. To simplify the solution, the organic solutes were lumped together as one single component. Consequently a pseudo one-component adsorption system is assumed. A differential material balance applied to the

The text was submitted by the authors in English.

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ARIBIKE, OLAFADEHAN

adsorbate carried by the following uid stream gives the following: C C C i ------- = D L1 ---------i U f -------i 2 z t z
2

1 b 3 ------------ --- K fi ( C i X i ) b R

(1) .

r=R

The initial and boundary conditions required to solve Eq. (1) are: (i) Ci = Coi, (t = 0, 0 z zT), (2) (ii) U f C oi ( t ) U f C i C (iii) -------i z = 0,
z = zT z=0

C + D L1 -------i z

= 0, ( t > 0 ), (3)
z=0

Equations (1)(8) are normally expressed for each of the components (pollutants) in a multicomponent adsorption system. The system under consideration is multicomponent as it involves the removal of phenolic compounds from wastewater. However, the complex multicomponent adsorption system was rationalized into a single system, which is simpler and easier to handle mathematically than a multicomponent system. The latter is a pseudo single-component adsorption system in which the phenolic compounds have been lumped into one single component. In the experimental work of Olafadehan and Aribike [21], the concentrations of the pollutants were lumped together as chemical oxygen demand. The latter decision was hinged on the fact that the industrial wastewater employed in the experiment was found to contain mainly phenols. NUMERICAL METHOD OF SOLUTION The numerical method of solution of the partial differential equations (1) and (5) is the method of orthogonal or optimal collocation. The orthogonal collocation method is applied by rst choosing a new set of dimensionless variables which have values lying between 0 and 1. The following dimensionless variables are dened: r = -----; 2 R
2

( t > 0 ).

(4)

The differential mass balance for the adsorbate in the pore uid is given by p 2 X X ---- ---- r D pi -------i + f ri = p -------i - 2 r r t r +

j=1

X i q * --------j ------- X j t

(5)

subject to the initial and boundary conditions: (i) X i = 0, ( t = 0, 0 < r < R, 0 z z T ), = K fi ( C i X i ),

r=R

tD pi = --------- ; A Ci C i = ------ ; C oi zT U f Pe 1 = ----------- ; D L1

A = R ;
2

(6)

X p D pi -------i r (ii) X (iii) -------i r

z Z = ----; zT q i* Q i* = ----- ; * q oi

Xi X i = ------ ; C oi 2RK fi Sh i = -------------- . p D pi

(7)

( 0 z z T, 0 < r < R, t > 0 ), = 0,

r=R

( 0 z z T, 0 < r < R, t > 0 ). (8)

The transformed equations for a one-component system for the uid phase and pore-uid phase with no chemical reaction are respectively given by C 1 C1 C 1 -------- = 1 -------- + 2 ---------- 3 ( C 1 X 1 ) 2 Z Z
2 =1

The above model equations are nonlinear partial differential equations (PDE), second order with respect to z (axial distance) and rst order with respect to time, t. These equations are applicable to the adsorption of organic pollutants from wastewater using a xed bed of adsorbent material in conjunction with an appropriate adsorption isotherm. An earlier experimental study by the same authors [21] revealed that the equilibrium data for the system was adequately correlated by the Freundlich adsorption isotherm at a temperature of 25C and pressure of 1 atm. This clearly indicates that the nonlinear adsorption isotherm of Freundlich is suitable and applicable to the adsorption of phenolic compounds on granular activated carbon in a xed bed; hence, its use in this study is justied. The Freundlich adsorption isotherm is given by q* = i
n a fi X i i .

, (10)

2 pA X1 X1 X1 1 -------- = -------- 4 ---------- + 6 -------- , 2 R2

(11)

where UfA 1 = ------------- , z T D p1 1 UfA 2 = ---------------------- = --------, Pe 1 z T Pe 1 D p1

1 b 3 K f 1 A 3 = ------------ --- ------------ , b R D p1 q * Q * o1 1 1 = p + ------- ---------- C o1 X 1

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subject to the transformed initial and boundary conditions: (i) C 1 = 1, ( 0 z 1, 0 ), ,

Z=0

Also, upon application of orthogonal collocation to the system model equation for the spherical particle radial direction, Eq. (11) becomes d X 1, j p A ------------ = ----------- 4 j 2 d 1 R
NR + 1

(12) ( > 0 ), (13)

1 C 1 (ii) C 1 ( 0, ) = 1 + -------- -------- Pe 1 Z C 1 (iii) -------- Z = 0,

Z=1

NR + 1

B j, k X 1, k + 6

k=1

k=1

A j, k X 1, k , (23)

( j = 1, 2, , NR ), (14) (15) subject to X 1, j = 0, j = 1, 2, , NR + 1, 0, (24)

( > 0 ),

(iv) X 1 = 0, 4 X1 ------- -------- Sh 1 (v)

( 0 1, 0 ), = ( C1 X 1 )
=1 =1

(16)

4 ------- Sh 1

NR + 1

k=1

A N + 1, k X 1, k = C 1, j X 1, N + 1 ,

(25)

( 0 Z 1, > 0 ), X1 (vi) -------- = 0,

=0

j = 2, 3, , NR + 1, > 0, where NR is the number of collocation points in the radial direction inside the catalyst particle. It should be noted that the boundary points Z = 0 and Z = 1 are taken as external collocation points in Eq. (10), whereas only the boundary point = 1 is taken as an external collocation point. Equations (21) and (22) were used to reduce the number of terms in the summations in Eq. (19) such that it is taken from k = 2 to k = N + 1 by the following procedure. First, Eqs. (21) and (22) were solved for C 1, 1 and C 1, N + 2 to obtain the following expressions:
N+1

( 0 Z 1, > 0 ).

(17)

Using the Freundlich adsorption isotherm for a onecomponent system, the appropriate dimensionless variable 1 is then given by 1 = p + a f 1 n 1 ( C o1 X 1 )
n1 1

(18)

Equations (10) and (11) with their respective initial and boundary conditions represent a set of two coupled nonlinear PDEs, which can only be solved numerically. When the method of orthogonal collocation is applied to Eq. (10) becomes this equation dC 1, j B j, k C 1, k 1 A j, k C 1, k ------------ = 2 d k = 1 k = 1
N+2

C 1, 1 = Pe '1 +

A'
N+1

1, k C 1, k ,

(26)

k=2

N+2

(19) where

C 1, N + 2

= Pe '' + 1

A''

1, k C 1, k ,

(27)

k=2

3 ( C 1, j X 1, N + 1 ),

( j = 2, 3, , N + 1 ),

where N is the number of interior collocation points in the axial direction. The two extra points have been included to incorporate the boundary points at the inlet and outlet of the xed bed reactor. The initial and boundary conditions are transformed as follows: C 1, j = 1, ( j = 1, 2, , N + 2, 0 ),
N+2

Pe 1 --------------A 1, N + 2 Pe '1 = ---------------------------------------------------------------------, Pe 1 A 1, 1 A N + 2, 1 --------------- --------------- + ---------------------A 1, N + 2 A 1, N + 2 A N + 2, N + 2 A N + 2, k A 1, k --------------- ---------------------A 1, N + 2 A N + 2, N + 2 = ---------------------------------------------------------------------, Pe 1 A 1, 1 A N + 2, 1 --------------- --------------- + ---------------------A 1, N + 2 A 1, N + 2 A N + 2, N + 2

(28)

(20)

A '1, k

(29)

1 C 1, 1 = 1 + -------- A 1, k C 1, k , Pe 1 k=1

( Z = 0, > 0 ), (21)

N+2

A N + 2, k C 1, k = 0,

(Z = 1, > 0),

(22)

k=1

Pe 1 ----------------------A 1, 1 Pe 1 Pe '' = ----------------------------------------------------- , 1 A 1, N + 2 A N + 2, N + 2 ---------------------- ----------------------A N + 2, 1 A 1, 1 Pe 1

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ARIBIKE, OLAFADEHAN

A '', k 1

A N + 2, A 1, k ----------------------- ---------------k A 1, 1 Pe 1 A N + 2, 1 = ----------------------------------------------------- . A 1, N + 2 A N + 2, N + 2 ---------------------- ----------------------A N + 2, 1 A 1, 1 Pe 1

4 = 1 ( 4 j B j, N + 1 + 6 A j, N + 1 ). (31)

(41)

Also, Eq. (25) was used to reduce the sums in Eq. (23) such that they were taken from k = 1 to k = NR to yield Eq. (32), which was then used to eliminate X 1, N+1 from Eq. (19): X 1, N + 1 = 1 C 1, j where 1 1 = -----------------------------------------, 4 1 + ------- A N + 1, N + 1 Sh 1 4 A 'N + 1, k = ------- A N + 1, k 1 . Sh 1 (33)

A'
k=1

NR

N + 1, k X 1, k ,

(32)

In Eq. (39), the concentrations corresponding to = 1 have been eliminated. Thus, the problem has now been reduced to solving simultaneously the set of nonlinear, coupled, stiff differential equations (35) and (39), and the initial conditions given by Eqs. (20) and (24) using the Freundlich isotherm. Equations (35) and (39) constitute 2N equations in 2N unknown concentrations (exclusive of the initial concentrations). This set of equations was integrated using the semi-implicit RungeKutta routine combined with step-size adjustment strategy. SIMULATION RESULTS AND DISCUSSION The equilibrium isotherms determined for the adsorption of phenolic compounds on granular activated carbon at 25C and 1 atm have the following forms [21]: For sample A, q * = 33.2613 X A A
1.7547

(34)

(42) (43) (44)

Use of Eqs. (26) and (27) to eliminate the concentrations at Z = 0 and Z = 1 ( C 1, 1 , C 1, N + 2 ) from Eq. (19) results in a reduction of the number of terms in the summations. After the above substitutions have been made, the summations in Eq. (19) run from k = 2 to k = N + 1. The resulting equation for the uid phase is given thus: dC 1, j ------------ = d
N+1

8.5343 For sample B, q * = 10.6474 X B . B

For sample C, q * = 2.3181 X C C

1.7667

j, k C 1, k

A'
k=1

NR

N + 1, k X 1, k

k=1

(35)

+ 1 C 1, j + Pe 1 , where T j, k = 2 ( B j, N + 2 A '', k + B j, 1 A '1, k + B j, k ) 1 1 ( A j, N + 2 A '', k + A j, 1 A '1, k + A j, k ), 1 1 = 3 ( 1 1 ), '' ' Pe 1 = 2 ( B j, N + 2 Pe 1 + B j, 1 Pe 1 ) 1 ( A j, N + 2 Pe '' + A j, 1 Pe '1 ), 1 (36) (37) (38)

Use of Eq. (32) to eliminate X 1, N+1 from Eq. (23) yields the following expression having summations ranging from k = 1 to k = NR: pA d X 1, ------------j = ----------- U j, k X 1, k + 4 C 1, j , 2 d 1 R k = 1

NR

(39)

where U j, k = 4 j ( B j, k B j, N + 1 A 'N + 1, k ) + 6 ( A j, k A j, N + 1 A 'N + 1, k ), (40)

The {Aj, k} and {Bj, k} were evaluated on the basis of power series in the concentrations, and the weighting function, W(x) = (1 x)x = (1 x)0x0 = 1. This value of W(x) gives faster convergence [14]. The approximation orders, N and NR, of the orthogonal polynomials ( 0, 0 ) ( 0, 0 ) P N (Z) and P NR (y) for the equations of the moving uid and micropore diffusion, respectively, were each equal to eight since this has proved to be sufcient to obtain differences in only the fourth digit as compared to the higher and lower approximations [15], thereby justifying the use of only eight collocations points. In the column calculations of this study, the value of the pore diffusivity, Dp1, was taken to be constant since extensive column calculations using the pore diffusion model have shown the results to be less sensitive than those of the nite bath for moderate changes in the values of the pore diffusivity [22]. The value of the axial dispersion coefcient, DL1, was calculated using the correlation developed by Liles and Geankoplis [23]. The lm mass transfer coefcient, Kf1, was calculated using the correlation developed by Wilson and Geankoplis [24] and Mandelbaum and Bohm [25], which are appropriate at low Reynolds numbers. In this pseudo monocomponent adsorption system, the Reynolds numbers are 0.96 and 1.91 for particle sizes of 12 mm and >2 mm, respectively. Both correlations gave almost the same set of values for the lm mass transfer coefcient. If the Wilke and Hougen correlation [26] is used to calculate the lm mass transfer coefcient, the value obtained is 28.5% higher than that obtained using the correlation of either Wilson and Geankoplis [24] or Mandelbaum and Bohm [25]. This is indicative of the
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inappropriateness of the Wilke and Hougen correlation [26] at low Reynolds numbers. The calculated values of the axial diffusion coefcient and the lm mass transfer coefcient are given thus: DL1 = 4.0 106 m2/s and Kf1 = 2.12 105 m/s. Other parameter values used in the column calculations are as follows: p = 0.94; b = 0.4493 and 0.4459 for particle sizes of 12 mm and >2 mm, respectively; Uf = 4.6214 103 m/s; Co1 = 0.2419, 0.2727, and 0.0377 kg/m3 for samples A, B, and C, respectively; qo1 = 0; Dp1 = 7.40 1010 m2/s; R = 1.5 103 and 3.0 103 m for particle sizes of 12 mm and >2 mm, respectively; Dr = 0.02150 m; and zT = 0.64 and 0.42 m for particle sizes of 12 mm and >2 mm, respectively. The coefcients in the Freundlich isotherm are given in Eqs. (42)(44), that is, af1 = 33.2613, 10.6474, and 2.3181 for samples A, B, and C, respectively, and n1 = 0.57, 0.1172, and 0.5660 for samples A, B, and C, respectively. These values of constants and parameters were estimated in the experimental study performed by Olafadehan and Aribike [21] and to which the simulation results of the present work are compared. Figures 13 show the predicted complete breakthrough proles for phenolic compounds in the pseudo single-component adsorption system using particle sizes of 12 mm and >2 mm. The curves were smooth and sigmoidal and characterized by an initial low level of normalized concentration for sample C, which were then followed by a sharp and steep ascent to the exhaustion. Figures 13 also show the comparison between the experimental results of Olafadehan and Aribike [21] and the simulated results of the present study for GAC particle sizes of 12 mm and >2 mm. Statistical analyses of t are as follows for the average standard deviation of 0.0016, 0.0002, and 0.0002 for samples A, B, and C, respectively, using particle size of 12 mm, with their respective regression coefcients being 0.9950, 1.0006, and 0.9999. For particle size >2 mm, average standard deviation gave 0.0007, 0.0002, and 0.0030 for samples A, B, and C, respectively, with their respective regression coefcients being 0.9961, 0.9888, and 0.9909. Hence, it can be concluded that excellent agreement was achieved between the experimental data and the predicted results, without any attempt made to adjust the lm and axial dispersion coefcients taken from the literature. The effects of particle sizes on breakthrough curves for samples A, B, and C can also be seen in Figs. 13. It is revealed that a strong inuence occurs at early breakthrough times, observed to be the highest for >2 mm particle size for all three samples of wastewater efuents, and decreases for 12 mm particle size. Therefore, the particle sizes used in the column affect the breakthrough times. Breakthrough times of 40, 25, and 150 min, respectively, were predicted for phenolic compounds in wastewater samples A, B, and C for particle sizes of 12 mm. In the case of particle sizes greater than 2 mm, breakthrough times of 90, 90, and 160 min were obtained for A, B, and C, respectively. This indicates that it will take the carbon bed

Dimensionless exit concentration

0.25 0.20 0.15 0.10 0.05 0 50 100 150 200 250 300 350 400
Time, min Fig. 1. Predicted versus experimental breakthrough proles for phenolic compounds in sample A.
12 mm particle size (predicted) 12 mm particle size (experimental) 2 () 2 ()

Dimensionless exit concentration

0.20 0.18 0.16 0.14 0.12 0.10 0.08 0.06 0.04 0.02 0 50 100 150 200 250 300 350 400
Time, min Fig. 2. Predicted versus experimental breakthrough proles for phenolic compounds in sample B. Dimensionless exit concentration

0.8 0.7 0.6 0.5 0.4 0.3 0.2 0.1 0 50 100 150 200 250 300 350 400
Time, min Fig. 3. Predicted versus experimental breakthrough proles for phenolic compounds in sample C.

between 1 and 3 h to become saturated for the cases considered. The excellent agreement exhibited in this study has shown conclusively that a multicomponent adsorption system can be converted into a simple pseudo singlecomponent system by lumping concentrations of components into one, particularly when the components are of the same functional group. This step is plausible, as such components would have equal opportunity of
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Dimensionless solid concentration

ARIBIKE, OLAFADEHAN

0.25 0.20 0.15 0.10 0.05 0 0.02 0.04 0.06 0.08 0.10 0.12 0.14 0.16 0.18
Dimensionless liquid phase concentration Fig. 4. Relation between solid phase and bulk liquid phase concentrations for phenolic compounds in sample B: (1) 12 mm particles; (2) particles larger than 2 mm.

1 2

Dpidiffusivity for component i in the fluid phase within the pore of an adsorbent, m2/s; Drdiameter of reactor, m; Kfifilm mass transfer coefficient of solute i, m/s; Nnumber of interior collocation points in the axial direction; NRnumber of interior collocation points in the radial direction; Pe1Peclet number of component i, dimensionless; q * concentration of solute i in the solid (or i adsorbed) phase, kg/m3; q * concentration of adsorbed solute i at equiliboi rium when the uid phase concentration is Coi at z = 0, kg/m3; Rexternal radius of the adsorbent, m; rradial distance in particle (radius of the adsorbent pellet as measured from center of pellet), m; ShiSherwood number of component i, dimensionless; ttime from start of sorption process, s; Uflinear velocity in the positive direction of z, m/s; Xiconcentration of solute i in pore fluid phase, kg/m3; zaxial distance in column, m; zTlength of column, m. Greek Symbols bvoid fraction in the bed (i.e., volume of voids per unit volume of bed), dimensionless; pvoid fraction in particles (i.e., volume of pores in the pellet per unit volume of pellet), dimensionless; dimensionless radius (r2/R2); dimensionless time (tDpi/A). Dimensionless Parameters C i dimensionless concentration of solute i in uid phase of the column (Ci/Coi); Q i* dimensionless concentration of solute i in the solid (or adsorbed) phase ( q * / q * ); i oi X i dimensionless concentration of solute i in pore uid phase (XXi/Coi); Zdimensionless distance (z/zT). Superscript *equilibrium value.
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adsorbing onto available sites. In this case, shifting of sites, which normally arises during competitive adsorption, would not occur here. Shifting of sites occurs as a result of interaction amongst the components as described in the adsorption isotherms of Langmuir and Fritz and Schluender [27]. Figure 4 is typical of the relation between the solid phase and bulk liquid phase concentrations for phenolic compounds in wastewater samples A, B, and C. The plots revealed the formation of a primary monomolecular layer on the adsorption sites. CONCLUSIONS The multicomponent adsorption system dened for the removal of phenols from industrial wastewater was rationalized into a pseudo monocomponent adsorption system by lumping together the concentrations as one. It was shown that, in certain cases of a multicomponent adsorption system as in this study, it might not be necessary to solve the resulting complex model equations. Converting the latter to a simple pseudo monocomponent adsorption system and solving the resulting equation could be adequate. NOTATION aficonstant in Freundlich adsorption isotherm; Across-sectional area of the column, m2; Aj, kconstant generated in the orthogonal collocation method; Bj, kconstant generated in the orthogonal collocation method; Ciconcentration of solute i in fluid phase of the column, kg/m3; Coiinlet concentration of solute i in the column, kg/m3; DL1axial diffusivity for component i in the fluid phase, m2/s;

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Subscript i, jinteger value; Lliquid phase; ppore phase; ssolid phase. REFERENCES
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